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Heavy metal pollution in the environment has become a significant global concern due to its detrimental effects on human health and the environment. In this study, we report an electrochemical aptasensor for the simultaneous detection of Hg2+ and Pb2+. Gold nanoflower/polyethyleneimine-reduced graphene oxide (AuNFs/PEI-rGO) was introduced on the surface of a gold electrode to improve sensing performance. The aptasensor is based on the formation of a T-Hg2+-T mismatch structure and specific cleavage of the Pb2+-dependent DNAzyme, resulting in a dual signal generated by the Exo III specific digestion of methylene blue (MB) labeled at the 3' end of probe DNA-1 and the reduction of the substrate ascorbic acid (AA) catalyzed by the signal label. The decrease of MB signal and the increase of AA oxidation peak was used to indicate the content of Hg2+ and Pb2+, respectively, with detection limits of 0.11 pM (Hg2+) and 0.093 pM (Pb2+). The aptasensor was also used for detecting Hg2+ and Pb2+ in water samples with good recoveries. Overall, this electrochemical aptasensor shows promising potential for sensitive and selective detection of heavy metals in environmental samples.
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Aptámeros de Nucleótidos , Técnicas Biosensibles , Técnicas Electroquímicas , Exodesoxirribonucleasas , Plomo , Mercurio , Estructuras Metalorgánicas , Contaminantes Químicos del Agua , Mercurio/análisis , Plomo/análisis , Plomo/química , Estructuras Metalorgánicas/química , Aptámeros de Nucleótidos/química , Exodesoxirribonucleasas/química , Exodesoxirribonucleasas/metabolismo , Contaminantes Químicos del Agua/análisis , Técnicas Biosensibles/métodos , Grafito/química , Oro/química , Límite de Detección , Electrodos , ADN Catalítico/químicaRESUMEN
The voltage-gated ion channels, also known as ionic transistors, play substantial roles in biological systems and ion-ion selective separation. However, implementing the ultrafast switchable capabilities and polarity switching of ionic transistors remains a challenge. Here, we report a nanofluidic ionic transistor based on carbon nanotubes, which exhibits an on/off ratio of 104 at operational gate voltage as low as 1 V. By controlling the morphology of carbon nanotubes, both unipolar and ambipolar ionic transistors are realized, and their on/off ratio can be further improved by introducing an Al2O3 dielectric layer. Meanwhile, this ionic transistor enables the polarity switching between p-type and n-type by controlled surface properties of carbon nanotubes. The implementation of constructing ionic circuits based on ionic transistors is demonstrated, which enables the creation of NOT, NAND, and NOR logic gates. The ionic transistors are expected to have profound implications for low-energy consumption computing devices and brain-machine interfacing.
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Voltage-gated ion channels prevalent in neurons play important roles in generating action potential and information transmission by responding to transmembrane potential. Fabricating bio-inspired ionic transistors with ions as charge carriers will be crucial for realizing neuro-inspired devices and brain-liking computing. Here, we reported a two-dimensional nanofluidic ionic transistor based on a MXene membrane with sub-1â nm interlayer channels. By applying a gating voltage on the MXene nanofluidic, a transmembrane potential will be generated to active the ionic transistor, which is similar to the transmembrane potential of neuron cells and can be effectively regulated by changing membrane parameters, e.g., thickness, composition, and interlayer spacing. For the symmetric MXene nanofluidic, a high on/off ratio of ~2000 can be achieved by forming an ionic depletion or accumulation zone, contingent on the sign of the gating potential. An asymmetric PET/MXene-composited nanofluidic transitioned the ionic transistor from ambipolar to unipolar, resulting in a more sensitive gate voltage characteristic with a low subthreshold swing of 560â mV/decade. Furthermore, ionic logic gate circuits, including the "NOT", "NAND", and "NOR" gate, were implemented for neuromorphic signal processing successfully, which provides a promising pathway towards highly parallel, low energy consumption, and ion-based brain-like computing.
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Encéfalo , Nitritos , Elementos de Transición , Potenciales de Acción , Iones , Potenciales de la MembranaRESUMEN
The diagnosis and evaluation of traumatic brain injury (TBI) are crucial steps toward the treatment and prognosis of patients. A common question remains as to whether it is possible to introduce an ideal device for signal detection and evaluation that can directly connect digital signals with TBI, thereby enabling prompt response of the evaluation signal and sensitive and specific functioning of the detection process. Herein, a method is presented utilizing polymetric porous membranes with TRTK-12 peptide-modified nanochannels for the detection of S100B (a TBI biomarker) and assessment of TBI severity. The method leverages the specific bonding force between TRTK-12 peptide and S100B protein, along with the nanoconfinement effect of nanochannels, to achieve high sensitivity (LOD: 0.002 ng mL-1) and specificity (∆I/I0: 44.7%), utilizing ionic current change as an indicator. The proposed method, which is both sensitive and specific, offers a simple yet responsive approach for real-time evaluation of TBI severity. This innovative technique provides valuable scientific insights into the advancement of future diagnostic and therapeutic integration devices.
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Biomimética , Lesiones Traumáticas del Encéfalo , Humanos , Péptidos , Lesiones Traumáticas del Encéfalo/diagnóstico , Pronóstico , Biomarcadores , Subunidad beta de la Proteína de Unión al Calcio S100RESUMEN
Despite being a clean and renewable energy source, photovoltaic (PV) power generation faces severe challenges in operation due to its strong intermittency and volatility compared to the traditional fossil fuel power generation. Accurate predictions are therefore crucial for PV's grid connections and the system security. The existing methods often rely heavily on weather forecasts, the accuracy of which is hard to be guaranteed. This paper proposes a novel GBDT-BiLSTM day-ahead PV forecasting model, which leverages the Teacher Forcing mechanism to combine the strong time-series processing capabilities of BiLSTM with an enhanced GBDT model. Given the uncertainty and volatility inherent in solar energy and weather conditions, the gradient boosting method is employed to update the weak learner, while a decision tree is incorporated to update the strong learner. Additionally, to explore the correlation between photovoltaic power output and historical time-series data, the adaptive gradient descent-based Adam algorithm is utilized to train the bidirectional LSTM model, enhancing the accuracy and stability of mid- to long-term time-series predictions. A prediction experiment, conducting with the real data from a PV power station in Sichuan Province, China, was compared with other methods to verify the model's effectiveness and robustness.
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Under the threat of energy crisis and environmental pollution, the technology for sustainable and clean energy extraction has received considerable attention. Owing to the intensive exploration of energy conversion strategies, expanded energy sources are successfully converted into electric energy, including mechanical energy from human motion, kinetic energy of falling raindrops, and thermal energy in the ambient. Among these energy conversion processes, charge transfer at different interfaces, such as solid-solid, solid-liquid, liquid-liquid, and gas-contained interfaces, dominates the power-generating efficiency. In this review, the mechanisms and applications of interfacial energy generators (IEGs) with different interface types are systematically summarized. Challenges and prospects are also highlighted. Due to the abundant interfacial interactions in nature, the development of IEGs offers a promising avenue of inexhaustible and environmental-friendly power generation to solve the energy crisis.
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Photocatalytic methane conversion requires a strong polarization environment composed of abundant activation sites with the robust stretching ability for C-H scissoring. High-density frustrated Lewis pairs consisting of low-valence Lewis acid Nb and Lewis base Nb-OH are fabricated on lamellar Nb2O5 through a thermal-reduction promoted phase-transition process. Benefitting from the planar atomic arrangement of lamellar Nb2O5, the frustrated Lewis pairs sites are highly exposed and accessible to reactants, which results in a superior methane conversion rate of 1456 µmol g-1 h-1 for photocatalytic non-oxidative methane coupling without the assistance of noble metals. The time-dependent DFT calculation demonstrates the photo-induced electron transfer from LA to LB sites enhances their intensities in a concerted way, promoting the C-H cleavage through the coupling of LA and LB. This work provides in-depth insight into designing and constructing a polarization micro-environment for photocatalytic C-H activation of methane without the assistance of noble metals.
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The abuse of chloramphenicol (CAP) in animal-derived products leads to serious food safety problems, so the sensitive and accurate determination of CAP residues has great noteworthiness for public health. Herein, we present a novel electrochemical aptasensor that incorporates a poly(diallyldimethylammonium chloride) functionalized graphene/Ag@Au nanosheets (PDDA-Gr/Ag@Au NSs) composite modified electrode and a DNAzyme signal amplification effect triggered by a triple-helix molecular switch (THMS) for detecting CAP. The PDDA-Gr/Ag@Au NSs composite has the advantages of high surface area, great conductivity, and dispersibility and has successfully improved the electrochemical performance of the electrode. Specific interaction with CAP will cause the signal transduction probe (STP) to be released from the THMS. After that, the DNAzyme will be activated with the help of Pb2+ and remove the immobilized signal probe on the electrode surface. The signal change was recorded by square wave voltammetry (SWV) and led to an accurate quantification of CAP. With all these features, the proposed sensing strategy yielded a satisfactory analytical performance with linearity between 1 pM and 1 µM and a limit of detection of 18.6 fM. Furthermore, the aptasensor shows excellent specificity for CAP in the presence of other antibiotics and resists interference with other common metal ions. Importantly, the performance is not diminished when the constructed aptasensor is applied to measuring CAP in milk powder. This THMS-based method is easy to design, and alteration to different targets can be achieved by simply replacing the aptamer sequence in the THMS. Therefore, this method shows significant prospects as a flexible platform for accurate monitoring of antibiotic residues in foodstuffs.
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Aptámeros de Nucleótidos , Técnicas Biosensibles , ADN Catalítico , Grafito , Nanopartículas del Metal , Animales , Antibacterianos , Aptámeros de Nucleótidos/química , Técnicas Biosensibles/métodos , Cloranfenicol/química , ADN Catalítico/química , Técnicas Electroquímicas/métodos , Oro/química , Grafito/química , Límite de Detección , Nanopartículas del Metal/químicaRESUMEN
Herein, a hierarchically porous Zr-MOF-labeled electrochemical aptasensor based on the composite of PtPd@Ni-Co hollow nanoboxes (PtPd@Ni-Co HNBs) and poly (diallyldimethylammonium chloride)-functionalized graphene (PDDA-Gr) was developed for ultrasensitive detection of chloramphenicol (CAP). PtPd@Ni-Co HNBs have excellent conductivity and provide binding sites for aptamers; the functionalized PDDA-Gr improves its dispersibility and conductivity as a substrate material, which can be successfully used to increase the electrode surface area and support more PtPd@Ni-CoHNBs. Besides, hierarchically porous Zr-MOFs (HP-UiO-66) were utilized as signal probes and showed a stronger load capacity for signal molecules than conventional UiO-66. In the presence of CAP, two ingeniously designed Exo III-assisted cyclic amplification strategies further improved the sensitivity of the aptasensor: CAP causes cycle I to release a large amount of trigger DNA (Tr DNA), and then, Tr DNA initiated cycle II, which causes the exposed capture DNA to further bind the signal probes. With these advantages, the constructed aptasensors performed with satisfactory sensitivity in a wide linear range (10 fM-10 nM) and a detection limit of 0.985 fM. Several signal amplification strategies adopted in this study have effectively improved the performance of the sensor, providing a new avenue for the development of ultrasensitive sensors in the food analysis field.
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Aptámeros de Nucleótidos/química , Técnicas Biosensibles/métodos , Cloranfenicol/análisis , Técnicas Electroquímicas/métodos , Electrodos , Exodesoxirribonucleasas/metabolismo , Miel/análisis , Nanopartículas del Metal/química , Grafito/química , Metales/química , Polietilenos/química , Compuestos de Amonio Cuaternario/químicaRESUMEN
An electrochemical aptasensor, including the polyethyleneimine-graphite-like carbon nitride/Au nanowire nanocomposite (PEI-C3N4/AuNWs) and exonuclease-assisted signal amplification strategy was constructed for the determination of chloramphenicol (CAP). Initially, a nanocomposite with substantial electrocatalytic property was synthesized by PEI-C3N4/AuNWs. This improves the conductivity and specific surface area of the PEI-C3N4/AuNW-modified gold electrode. Next, a DNA with a complementary sequence to a CAP aptamer (cDNA) was immobilized on the PEI-C3N4/AuNW-modified electrode, followed by the CAP aptamer hybridized with cDNA. The lower signal at this time is due to the negatively charged phosphate group of the oligonucleotide and [Fe (CN)6]3-/4- electrostatically repelling each other. The presence of the CAP would cause aptamer on the electrode surface to fall off and be digested by Recjf exonuclease, which resulted in target recycling, and a significant increase in DPV signal can be observed at a potential of 0.176 V (vs. Ag/AgCl). Under optimal conditions, there is a linear relationship between the peak current and the logarithm of CAP concentration in the range 100 fM-1 µM, and the detection limit of this aptasensor is 2.96 fM (S/N = 3). Furthermore, the resultant aptasensor has excellent specificity, reproducibility, and long-term stability, and has been applied to the detection of CAP in milk samples. Graphical abstract The detection principle of the electrochemical aptasensor for CAP detection was based on PEI-C3N4/AuNWs and exonuclease-assistant signal amplification. It is based on the fact that PEI-C3N4/AuNWs nanocomposites on the surface of the electrode can effectively improve the performance of the aptasensor, and Recjf exonuclease initiates the target recycling process, causes signal amplification.